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PdAgRu nanoparticles on polybenzimidazole wrapped CNTs for electrocatalytic formate oxidation
Electrochimica Acta ( IF 5.5 ) Pub Date : 2020-07-04 , DOI: 10.1016/j.electacta.2020.136678
Tesfaye Tadesse Gebremariam , Fuyi Chen , Bo Kou , Longfei Guo , Bowei Pan , Qiao Wang , Zhen Li , Weiqi Bian

Direct formate fuel cells (DFFCs) have received great interest as potential candidates of power sources, and their viability primarily relies on exploration of efficient formate oxidation reaction (FOR) catalysts. Herein, we have prepared PdAgRu nanoparticles supported on polybenzimidazole wrapped carbon nanotubes (pCNTs), Pd6Ag3Ru1/pCNTs catalyst which displays remarkable mass activity of 4.7 A mgPd−1 and maintains current density of 0.71 A mg−1 after 5400 s of chronoamperometry test, which is 2.1 and 26.7 times better than that of commercial Pd/C catalyst, respectively. The performance improvement is attributed to delicately designed components, polybenzimidazole layer serves as hydroxide transporter, carbon nanotubes function as electron conductive path, Ag weakens binding strength of adsorbed hydrogen (Hads) on Pd, and Ru promotes the formation of hydroxyl species. Impressively, when the upper limit potential of cyclic voltammetry is enlarged into Ag redox region, the FOR activity remarkably increases, the mass activities are 4.30, 4.7 and 5.12 A mgPd−1at 1.1, 1.3 and 1.5 V, respectively. The closer examination of x-ray photoelectron spectroscopy (XPS) spectra reveal the co-existence of mixed Pd(0)/Pd(II) and Ag(0)/Ag(I) state on the catalyst surface. The amount of Pd(0) and Ag(I) state increase with increasing upper limit potential, which is attributed to surface restructuration.



中文翻译:

聚苯并咪唑包裹的CNT上的PdAgRu纳米颗粒用于电催化甲酸氧化

直接甲酸燃料电池(DFFC)作为潜在的动力源已引起人们极大的兴趣,其可行性主要取决于对有效甲酸氧化反应(FOR)催化剂的探索。本文中,我们制备了负载在聚苯并咪唑包裹的碳纳米管(pCNTs)上的PdAgRu纳米颗粒,Pd 6 Ag 3 Ru 1 / pCNTs催化剂,该催化剂表现出显着的4.7 A mgPd -1的质量活度,并保持0.71 A mg -1的电流密度经过5400 s的计时电流法测试,分别比市售Pd / C催化剂高2.1倍和26.7倍。性能的提高归因于精心设计的组件,聚苯并咪唑层充当氢氧化物转运体,碳纳米管充当电子传导路径,Ag削弱了Pd上吸附的氢(H ads)的结合强度,Ru促进了羟基物种的形成。令人印象深刻的是,当循环伏安法的上限电位扩大到Ag氧化还原区域时,FOR活性显着增加,质量活性为4.30、4.7和5.12 A mgPd -1分别为1.1、1.3和1.5V。对X射线光电子能谱(XPS)光谱的仔细检查发现,催化剂表面上的Pd(0)/ Pd(II)和Ag(0)/ Ag(I)混合态共存。Pd(0)和Ag(I)态的数量随上限电位的增加而增加,这归因于表面重组。

更新日期:2020-07-08
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